WO2014096779A1 - Réacteur chimique multi-canaux - Google Patents

Réacteur chimique multi-canaux Download PDF

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Publication number
WO2014096779A1
WO2014096779A1 PCT/GB2013/053264 GB2013053264W WO2014096779A1 WO 2014096779 A1 WO2014096779 A1 WO 2014096779A1 GB 2013053264 W GB2013053264 W GB 2013053264W WO 2014096779 A1 WO2014096779 A1 WO 2014096779A1
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WIPO (PCT)
Prior art keywords
reactor
channel
temperature
block
flow channels
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PCT/GB2013/053264
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English (en)
Inventor
Tuan Quoc Ly
Robert Peat
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Compactgtl Limited
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Publication date
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Publication of WO2014096779A1 publication Critical patent/WO2014096779A1/fr

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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J19/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J19/0093—Microreactors, e.g. miniaturised or microfabricated reactors
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J19/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J19/24—Stationary reactors without moving elements inside
    • B01J19/248—Reactors comprising multiple separated flow channels
    • B01J19/249—Plate-type reactors
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
    • C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
    • C01B3/32—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air
    • C01B3/34—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents
    • C01B3/38—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by reaction of gaseous or liquid organic compounds with gasifying agents, e.g. water, carbon dioxide, air by reaction of hydrocarbons with gasifying agents using catalysts
    • C01B3/386—Catalytic partial combustion
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/00781—Aspects relating to microreactors
    • B01J2219/00783—Laminate assemblies, i.e. the reactor comprising a stack of plates
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/00781—Aspects relating to microreactors
    • B01J2219/00783—Laminate assemblies, i.e. the reactor comprising a stack of plates
    • B01J2219/00786—Geometry of the plates
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/00781—Aspects relating to microreactors
    • B01J2219/00819—Materials of construction
    • B01J2219/00822—Metal
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/00781—Aspects relating to microreactors
    • B01J2219/00819—Materials of construction
    • B01J2219/00835—Comprising catalytically active material
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/00781—Aspects relating to microreactors
    • B01J2219/00851—Additional features
    • B01J2219/00858—Aspects relating to the size of the reactor
    • B01J2219/0086—Dimensions of the flow channels
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/00781—Aspects relating to microreactors
    • B01J2219/00873—Heat exchange
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/00781—Aspects relating to microreactors
    • B01J2219/0095—Control aspects
    • B01J2219/00952—Sensing operations
    • B01J2219/00954—Measured properties
    • B01J2219/00961—Temperature
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/24—Stationary reactors without moving elements inside
    • B01J2219/2401—Reactors comprising multiple separate flow channels
    • B01J2219/245—Plate-type reactors
    • B01J2219/2451—Geometry of the reactor
    • B01J2219/2453—Plates arranged in parallel
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/24—Stationary reactors without moving elements inside
    • B01J2219/2401—Reactors comprising multiple separate flow channels
    • B01J2219/245—Plate-type reactors
    • B01J2219/2451—Geometry of the reactor
    • B01J2219/2456—Geometry of the plates
    • B01J2219/2459—Corrugated plates
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/24—Stationary reactors without moving elements inside
    • B01J2219/2401—Reactors comprising multiple separate flow channels
    • B01J2219/245—Plate-type reactors
    • B01J2219/2461—Heat exchange aspects
    • B01J2219/2462—Heat exchange aspects the reactants being in indirect heat exchange with a non reacting heat exchange medium
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/24—Stationary reactors without moving elements inside
    • B01J2219/2401—Reactors comprising multiple separate flow channels
    • B01J2219/245—Plate-type reactors
    • B01J2219/2461—Heat exchange aspects
    • B01J2219/2465—Two reactions in indirect heat exchange with each other
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/24—Stationary reactors without moving elements inside
    • B01J2219/2401—Reactors comprising multiple separate flow channels
    • B01J2219/245—Plate-type reactors
    • B01J2219/2476—Construction materials
    • B01J2219/2477—Construction materials of the catalysts
    • B01J2219/2479—Catalysts coated on the surface of plates or inserts
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/24—Stationary reactors without moving elements inside
    • B01J2219/2401—Reactors comprising multiple separate flow channels
    • B01J2219/245—Plate-type reactors
    • B01J2219/2476—Construction materials
    • B01J2219/2477—Construction materials of the catalysts
    • B01J2219/2481—Catalysts in granular from between plates
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/24—Stationary reactors without moving elements inside
    • B01J2219/2401—Reactors comprising multiple separate flow channels
    • B01J2219/245—Plate-type reactors
    • B01J2219/2476—Construction materials
    • B01J2219/2483—Construction materials of the plates
    • B01J2219/2485—Metals or alloys
    • B01J2219/2486—Steel
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
    • B01J2219/24—Stationary reactors without moving elements inside
    • B01J2219/2401—Reactors comprising multiple separate flow channels
    • B01J2219/245—Plate-type reactors
    • B01J2219/2491—Other constructional details
    • B01J2219/2497—Size aspects, i.e. concrete sizes are being mentioned in the classified document
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/02—Processes for making hydrogen or synthesis gas
    • C01B2203/0205—Processes for making hydrogen or synthesis gas containing a reforming step
    • C01B2203/0227—Processes for making hydrogen or synthesis gas containing a reforming step containing a catalytic reforming step
    • C01B2203/0233—Processes for making hydrogen or synthesis gas containing a reforming step containing a catalytic reforming step the reforming step being a steam reforming step
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/06—Integration with other chemical processes
    • C01B2203/062—Hydrocarbon production, e.g. Fischer-Tropsch process
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/08—Methods of heating or cooling
    • C01B2203/0805—Methods of heating the process for making hydrogen or synthesis gas
    • C01B2203/0811—Methods of heating the process for making hydrogen or synthesis gas by combustion of fuel
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/08—Methods of heating or cooling
    • C01B2203/0805—Methods of heating the process for making hydrogen or synthesis gas
    • C01B2203/0811—Methods of heating the process for making hydrogen or synthesis gas by combustion of fuel
    • C01B2203/0822—Methods of heating the process for making hydrogen or synthesis gas by combustion of fuel the fuel containing hydrogen
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/12—Feeding the process for making hydrogen or synthesis gas
    • C01B2203/1205—Composition of the feed
    • C01B2203/1211—Organic compounds or organic mixtures used in the process for making hydrogen or synthesis gas
    • C01B2203/1235—Hydrocarbons
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/16—Controlling the process
    • C01B2203/1614—Controlling the temperature
    • C01B2203/1619—Measuring the temperature
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B2203/00—Integrated processes for the production of hydrogen or synthesis gas
    • C01B2203/16—Controlling the process
    • C01B2203/1695—Adjusting the feed of the combustion
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P20/00—Technologies relating to chemical industry
    • Y02P20/10—Process efficiency

Definitions

  • the present invention relates to a chemical reactor, particularly but not exclusively a chemical reactor in which an exothermic reaction occurs.
  • the invention also relates to the control of a reaction taking place in such a chemical reactor. It would be relevant, for example, to a plant and a process for treating natural gas to produce a liquid product.
  • associated gas natural gas
  • associated gas natural gas
  • the gas can be transported to an off- site processing facility.
  • oil production takes place in more remote places it is difficult to introduce the associated gas into existing gas transportation infrastructure.
  • the associated gas has typically been disposed of by flaring or re-injection.
  • flaring the gas is no longer environmentally acceptable, while re- injection can have a negative impact on the subsequent quality of the oil from the well.
  • Gas-to-liquids technology can be used to convert the natural gas into liquid hydrocarbons and may follow a two-stage approach to hydrocarbon liquid production comprising syngas generation, followed by Fischer-Tropsch synthesis.
  • syngas a mixture of hydrogen and carbon monoxide
  • syngas may be generated by one or more of partial oxidation, auto-thermal reforming, or steam methane reforming.
  • steam methane reforming the reforming reaction is endothermic and so requires heat, and a catalyst such as platinum/rhodium; the heat may be provided by a combustion reaction.
  • the syngas is then subjected to Fischer-Tropsch synthesis, for which a suitable catalyst is cobalt on a ceramic support, and which is an exothermic reaction.
  • steam/methane reforming and Fischer-Tropsch synthesis may include a stack of plates shaped to define first and second sets of flow paths: an exothermic reaction may take place in one set of flow paths, and an endothermic reaction (or a coolant) be provided in the other set of flow paths.
  • an exothermic reaction may take place in one set of flow paths
  • an endothermic reaction or a coolant
  • a reactor comprising a reactor block having a plurality of alternately arranged flow channels, wherein the plurality of flow channels are arranged such that fluids in at least two adjacent flow channels can exchange heat through an intervening wall, and wherein the intervening wall defines at least one channel extending within the reactor block and communicating with an outside surface of the block and dimensioned to accommodate a temperature sensor.
  • the reactor may comprise a reactor block defining multiple first and second flow channels, the first and second flow channels being arranged alternately within the block and separated by intervening walls, such that fluids in the first and second flow channels can exchange heat through the intervening walls, wherein at least some of the intervening walls define at least one channel extending within the thickness of the wall and communicating with an outside surface of the block, to accommodate a temperature sensor.
  • the reactor block may comprise a stack of metal sheets that are arranged to define the first and second flow channels, the first and second flow channels being arranged alternately within the stack.
  • a catalyst may be provided in each flow-channel in which a chemical reaction is to be performed.
  • the catalyst may be coated onto the walls of the flow channel, or be provided in discrete pellets, such as extrudates or spheres, or as particles or powders, packed within the channel, or may be provided on gas-permeable non-structural elements.
  • the first and second flow channels may be defined by grooves in plates arranged as a stack, or by spacing strips and plates in a stack, the stack then being bonded together.
  • the flow channels may be defined by thin metal sheets that are castellated and stacked alternately with flat sheets; the edges of the flow channels may be defined by sealing strips.
  • the stack of plates forming the reactor may be bonded together for example by diffusion bonding, brazing, or hot isostatic pressing.
  • the temperature sensor is preferably selected to be suitable for operation at the temperature at which the reactor block is expected to operate, and one such temperature sensor is a thermocouple.
  • a temperature sensor within a flow channel may disrupt the flow; and replacing such a temperature sensor may be inconvenient or impractical. Since heat is transferred between the fluids in the first flow channels and the second flow channels, there is a temperature difference between the first flow channels and the second flow channels, and a temperature gradient through the intervening wall.
  • the temperature sensor can be removed and replaced during operation of the reactor.
  • the rate of reaction may increase as the temperature increases; and in such a case there is a positive feedback between the reaction rate and the temperature within the reactor.
  • This can lead to a rapid increase of temperature, referred to as a thermal runaway, and this can result in damage to the catalyst or to the reactor, or both, and would reduce the useful life of the reactor. It is therefore advantageous to monitor the performance of the reactor on a continuous basis, and to adjust the flow rates of any reactants in such a way as to prevent thermal runaway.
  • first and second flow channels for first and second fluids
  • the reactor block might define flow channels for more than two different fluids.
  • both the first and the second flow channels may be between 20 mm and 1 mm high (in cross-section); and each channel may be of width between about 1 .5 mm and 25 mm.
  • the plates in plan view
  • the flow channels are preferably of height between 2 mm and 10 mm (depending on the nature of the chemical reaction).
  • the plates might be 0.5 m wide and 1 .0 m long, or 0.6 m wide and 0.8 m long; and they may for example define channels 7 mm high and 6 mm wide, or 3 mm high and 10 mm wide, or 10 mm high and 5 mm wide.
  • Arranging the first and second flow channels to alternate in the stack helps ensure good heat transfer between fluids in those channels.
  • the first flow channels may be those for combustion (to generate heat) and the second flow channels may be for steam/methane reforming (which requires heat).
  • catalyst structures may be inserted into the channels, and may be removed for replacement. At least in some cases the catalyst structures are nonstructural, and do not provide strength to the reactor, so the reactor itself must be sufficiently strong to resist any pressure forces or thermal stresses during operation.
  • each such catalyst structure may be shaped so as to subdivide the flow channel into a multiplicity of parallel flow sub-channels.
  • Each catalyst structure may include a ceramic support material on the metal substrate, which provides a support for the catalyst.
  • the metal substrate provides strength to the catalyst structure and enhances thermal transfer by conduction.
  • the metal substrate may be of a steel alloy that forms an adherent surface coating of aluminium oxide when heated, for example a ferritic steel alloy that incorporates aluminium (eg Fecralloy (TM)), although the metal substrate may alternatively be of a different material such as stainless steel or aluminium, depending on the temperature and the chemical environment to which it is to be exposed.
  • TM Fecralloy
  • the substrate may be a foil, a wire mesh or a felt sheet, which may be corrugated, dimpled or pleated; the preferred substrate is a thin metal foil for example of thickness no more than 200 ⁇ , which is corrugated to define the longitudinal subchannels.
  • a flame arrestor is preferably provided at the inlet to each flow channel for combustion to ensure a flame cannot propagate back into the combustible gas mixture being fed to the combustion channel. This may be within an inlet part of each combustion channel, for example in the form of a non-catalytic insert that subdivides a portion of the combustion channel adjacent to the inlet into a multiplicity of narrow flow paths which are no wider than the maximum gap size for preventing flame propagation.
  • non-catalytic insert may be a longitudinally-corrugated foil or a plurality of longitudinally-corrugated foils in a stack.
  • a flame arrestor may be provided within the header.
  • the channels may be square in cross-section, or may be of height either greater than or less than the width; the height refers to the dimension in the direction of the stack, that is in the direction for heat transfer.
  • the catalyst element may for example comprise a single shaped foil, for example a corrugated foil; this is particularly suitable where the channel's minimum cross-sectional dimension is no more than about 3 mm, although it is also applicable in wider channels.
  • the catalyst structure may comprise a plurality of such shaped foils separated by substantially flat foils.
  • the combustion channels are preferably less than 10 mm high.
  • the channels are preferably at least 1 mm high, or it becomes difficult to insert the catalyst structures, and engineering tolerances become more critical.
  • the channels might all be 7 mm high and 6 mm wide, and in each case the catalyst element may comprise a single shaped foil, or a plurality of shaped foils.
  • Figure 1 shows a schematic perspective view, partly in section, of part of a reactor block suitable for steam/methane reforming
  • Figure 2 shows a perspective view of one of the plates forming the reactor block of figure 1 ;
  • Figure 3 shows a perspective view of a temperature sensor for use in the reactor block of figure 1 ;
  • Figure 4 shows graphically a temperature variation during operation of a steam/methane reforming reactor.
  • the invention would be applicable in a reactor for making synthesis gas, that is to say a mixture of carbon monoxide and hydrogen, from natural gas by steam reforming.
  • the synthesis gas may, for example, subsequently be used to make longer-chain hydrocarbons by a Fischer-Tropsch synthesis.
  • the steam reforming reaction is brought about by mixing steam and methane, and contacting the mixture with a suitable catalyst at an elevated temperature so the steam and methane react to form carbon monoxide and hydrogen.
  • the steam reforming reaction is endothermic, and the heat may be provided by catalytic combustion, for example of hydrocarbons and/or hydrogen mixed with air, so combustion takes place over a combustion catalyst within adjacent flow channels within the reforming reactor.
  • the reactor 5 includes a reactor block 10 which defines channels 16 for a catalytic combustion process and channels 17 for steam methane reforming.
  • the reactor block 10 consists of a stack of plates that are rectangular in plan view, each plate being of corrosion resistant high- temperature alloy such as Inconel 625, Incoloy 800HT or Haynes HR-120.
  • Flat plates 12 or 13 are arranged alternately with castellated plates 14 or 15, so the castellations define the channels 16 or 17.
  • the castellated plates 14 and 15 are arranged in the stack alternately.
  • the thickness of the castellated plates 14 and 15 is in each case 0.9 mm.
  • the height of the castellations is 3.9 mm in each case, and solid bars 18 of the same thickness are provided along the sides.
  • the wavelengths of the castellations in the castellated plates 14 and 15 may be different from each other, but as shown in the figure the wavelengths may be the same, so that in each case successive fins or ligaments are 10 mm apart.
  • the castellated plates 14 and 15 may be referred to as fin structures.
  • Each of the flat plates 12 is a single 2 mm-thick plate, whereas each of the flat plates 13 is formed of two flat plates 13a of thickness 1 mm that are bonded together.
  • the flat plates 13 are shown, but in practice the flat plates 13 would be provided at any height within the reactor block 10 at which the temperature is to be monitored. For example a reactor block might be made only using the flat plates 13, without any flat plates 12.
  • each of the flat plates 13a defines a groove 13b extending from one edge of the plate 13a, and in this case each groove 13b is of semicircular shape and of radius 0.55 mm.
  • the grooves 13b on adjacent surfaces of each pair of flat plates 13a are aligned with each other, so that the grooves 13b together define a straight channel 20 which, as shown in figure 1 , communicates with an outer surface of the reactor block 10.
  • a flat end plate 19 At each end of the stack is a flat end plate 19, which in this case is of thickness 4.0 mm.
  • the number of castellated plates 14 and 15 in the reactor block 10 is thirteen, so that the overall height of the reactor block 10 is 78.7 mm.
  • the stack of plates would be assembled and bonded together typically by diffusion bonding, brazing, or hot isostatic pressing.
  • a respective catalytic insert 22 or 24 (only one of each are shown in Figure 1 ), carrying a catalyst for the respective reaction, may be inserted into each channel 16 or 17.
  • These inserts 22 and 24 preferably have a metal substrate and a ceramic coating acting as a support for the active catalytic material, and the metal substrate may be a thin metal foil.
  • the insert 22, 24 may comprise a stack of corrugated foils and flat foils, or a single corrugated foil, occupying the respective flow channel 16 or 17, each foil being of thickness less than 0.1 mm, for example 50 ⁇ .
  • thermocouple 25 as shown in figure 3, of diameter 1 mm, can be installed into one or more of the channels 20.
  • the length of each thermocouple 25 is selected so that the end of the thermocouple 25 is at a position within the reactor block 10 where the temperature is to be measured.
  • the reactor block 10 is shown by way of example only.
  • the thickness of the plates 12 and 13 may be in the range 0.5 to 4 mm, and may differ from each other; while the thickness of the castellated plates 14 and 15 may be in the range 0.2 to 3.5 mm.
  • the heights of the castellations may be between 2 mm and 10 mm, and the separation between successive fins may be between 10 mm and 50 mm.
  • the channels 16 and 17 may instead be of height 6 mm and of width 7 mm.
  • the reactor block 10 may also be modified, for example in that the outermost channels, those adjacent to the end plate 19, may for example be blocked off so that no gases pass through them, hence reducing heat loss.
  • Other configurations for the reactor block 10 may be used according to the present invention.
  • the reactor block 10 may be formed by structures other than plates.
  • the metal of the plates 12, 13, 14 and 15 should not exceed 820 °C and that the braze which bonds them together should not exceed 815°C.
  • the temperature within the combustion channels 16 must be higher than that in the reforming channels 17, and there will be a temperature variation within each channel.
  • the temperature may be between 40° and 90 °C above that at the adjacent flat plate 12 or 13, while within the centre of a reforming channel 17 the temperature may be between 20° and 40 °C below that at the adjacent flat plate 12 or 13; this temperature difference will tend to be greater, the greater the height of the channel 16 or 17.
  • the fins separating adjacent channels 16 (or adjacent channel 17) will be at a lower temperature than at the centre of the channel 16 (or 17), because of heat transfer through the fin.
  • the metal within the fins separating adjacent combustion channels 16 may be at about 780 °C, and the flat plates 12 or 13 may be at about 770°C; within the combustion channels 16 the maximum gas temperature may be about 830 °C, while within the reforming channel 17 the maximum gas temperature may be about 740 °C.
  • the temperature at the catalyst insert 22 will rapidly increase; there is a time delay before the temperature at the adjacent flat plate 12 or 13 starts to increase; and a further time delay before the temperature in the adjacent reforming channel 17 starts to increase.
  • thermocouples 25 do not enable the maximum temperature within the combustion channels 16 to be measured, they do enable the temperature to be monitored in the vicinity of the brazed bonds, and so they enable the reactor 5 to be controlled in such a way that the safe operating temperatures are not exceeded.
  • FIG 4 shows graphically the variation in temperature, T, with time, t, in an experimental test carried out in such a steam/methane reforming reactor; and also shows the variation in fuel flow rate F.
  • the line A shows the variation of temperature within a plate 13 separating a combustion channel 16 from a reforming channel 17, as measured by a thermocouple 25 as described above.
  • the line B shows measurements of the temperature of the gas within the reforming channel 17, while the line C shows measurements of the temperature of the gas within the combustion channel 16.
  • the line D shows the variations in the fuel flow rate, F.
  • the time, t merely indicates the start of the graph; the observations were actually started after 1223 hours of operation.
  • the fuel flow rate, F is adjusted with the aim of maintaining a constant temperature.
  • thermocouple 25 within the plate 13 responds closely to combustion gas temperatures, so that by monitoring the temperature within the plate 13, changes in the temperature in the combustion channel 16 can be detected. Hence the thermocouples 25 enable the operation of a steam/methane reforming reactor 5 to be monitored and therefore controlled. If the temperature in the plate 13 rises more rapidly than desired, or rises to a higher temperature than desired, then the operation of the reactor 5 would be modified either by decreasing the supply of fuel to the combustion channels 16 or by increasing the flow of the

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  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Organic Chemistry (AREA)
  • Engineering & Computer Science (AREA)
  • Combustion & Propulsion (AREA)
  • Health & Medical Sciences (AREA)
  • General Health & Medical Sciences (AREA)
  • Inorganic Chemistry (AREA)
  • Hydrogen, Water And Hydrids (AREA)
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Abstract

La présente invention concerne un réacteur chimique (5) qui comprend un bloc de réacteur (10) définissant des premier et deuxième canaux d'écoulement multiples (16, 17) qui sont disposés de façon alternée à l'intérieur du bloc et séparés par des parois intermédiaires (12, 13), de sorte que des fluides dans les premier et deuxième canaux d'écoulement puissent échanger de la chaleur à travers les parois intermédiaires (12, 13). Au moins une partie des parois intermédiaires (13) définissent au moins un canal (20) s'étendant dans l'épaisseur de la paroi (30) et communiquant avec une surface extérieure du bloc (10), pour loger un capteur de température (25).
PCT/GB2013/053264 2012-12-17 2013-12-12 Réacteur chimique multi-canaux WO2014096779A1 (fr)

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GB2527847A (en) * 2014-07-04 2016-01-06 Compactgtl Ltd Catalytic reactors
EP3421122A1 (fr) * 2017-06-28 2019-01-02 Commissariat à l'Energie Atomique et aux Energies Alternatives Module de reacteur-echangeur a au moins deux circuits de fluide realise par empilement de plaques, applications aux reactions catalytiques exothermiques ou endothermiques
CN109634321A (zh) * 2018-12-31 2019-04-16 西安优耐特容器制造有限公司 适用于微反应实验的精确控温系统及方法
CN111412771A (zh) * 2019-01-08 2020-07-14 林德股份公司 用于制造板式热交换器的方法和具有热电偶或测量电阻器的板式热交换器
RU2796300C2 (ru) * 2019-01-08 2023-05-22 Линде Акциенгезелльшафт Способ изготовления пластинчатого теплообменника и пластинчатый теплообменник с термопарами или измерительными резисторами

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WO1995023914A1 (fr) * 1994-03-02 1995-09-08 Catalytica, Inc. Structure amelioree de catalyseur assurant un echange thermique integral
EP0848990A2 (fr) * 1996-12-21 1998-06-24 Degussa Aktiengesellschaft Réacteur pour effectuer des réactions catalytiques endothermes
WO2001041916A1 (fr) * 1999-12-08 2001-06-14 INSTITUT FüR MIKROTECHNIK MAINZ GMBH Systeme de microreaction modulaire
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GB2527847A (en) * 2014-07-04 2016-01-06 Compactgtl Ltd Catalytic reactors
WO2016001663A1 (fr) * 2014-07-04 2016-01-07 Compact Gtl Plc Réacteurs catalytiques à capteurs de température répartis
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CN106999898B (zh) * 2014-07-04 2020-02-14 康帕克特Gtl有限公司 包括分布式温度传感器的催化反应器
EP3421122A1 (fr) * 2017-06-28 2019-01-02 Commissariat à l'Energie Atomique et aux Energies Alternatives Module de reacteur-echangeur a au moins deux circuits de fluide realise par empilement de plaques, applications aux reactions catalytiques exothermiques ou endothermiques
FR3068263A1 (fr) * 2017-06-28 2019-01-04 Commissariat A L'energie Atomique Et Aux Energies Alternatives Module de reacteur-echangeur a au moins deux circuits de fluide realise par empilement de plaques, applications aux reactions catalytiques exothermiques ou endothermiques
CN109634321A (zh) * 2018-12-31 2019-04-16 西安优耐特容器制造有限公司 适用于微反应实验的精确控温系统及方法
CN109634321B (zh) * 2018-12-31 2021-02-05 西安优耐特容器制造有限公司 适用于微反应实验的精确控温系统及方法
CN111412771A (zh) * 2019-01-08 2020-07-14 林德股份公司 用于制造板式热交换器的方法和具有热电偶或测量电阻器的板式热交换器
EP3680599B1 (fr) 2019-01-08 2021-08-18 Linde GmbH Procédé de fabrication d'un échangeur de chaleur à plaques ainsi qu'échangeur de chaleur à plaques pourvu d'éléments thermiques ou de résistances de mesure
RU2796300C2 (ru) * 2019-01-08 2023-05-22 Линде Акциенгезелльшафт Способ изготовления пластинчатого теплообменника и пластинчатый теплообменник с термопарами или измерительными резисторами

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